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Water-Based Synthesis and Enhanced CO2 Capture Performance of Perfluorinated Cerium-Based Metal–Organic Frameworks with UiO-66 and MIL-140 Topology
Roberto D’Amato, Anna Donnadio, Mariolino Carta , Claudio Sangregorio, Davide Tiana, Riccardo Vivani, Marco Taddei , Ferdinando Costantino
ACS Sustainable Chemistry & Engineering
Swansea University Authors: Mariolino Carta , Marco Taddei
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DOI (Published version): 10.1021/acssuschemeng.8b03765
Reaction of cerium ammonium nitrate and tetrafluoroterephthalic acid in water afforded two new metal–organic frameworks with UiO-66 [F4_UiO-66(Ce)] and MIL-140 [F4_MIL-140A(Ce)] topologies. The two compounds can be obtained in the same experimental conditions, just by varying the amount of acetic ac...
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Reaction of cerium ammonium nitrate and tetrafluoroterephthalic acid in water afforded two new metal–organic frameworks with UiO-66 [F4_UiO-66(Ce)] and MIL-140 [F4_MIL-140A(Ce)] topologies. The two compounds can be obtained in the same experimental conditions, just by varying the amount of acetic acid used as crystallization modulator in the synthesis. Both F4_UiO-66(Ce) and F4_MIL-140A(Ce) feature pores with size <8 Å, which classifies them as ultramicroporous. Combination of X-ray photoelectron spectroscopy and magnetic susceptibility measurements revealed that both compounds contain a small amount of Ce(III), which is preferentially accumulated near the surface of the crystallites. The CO2 sorption properties of F4_UiO-66(Ce) and F4_MIL-140A(Ce) were investigated, finding that they perform better than their Zr-based analogues. F4_MIL-140A(Ce) displays an unusual S-shaped isotherm with steep uptake increase at pressure <0.2 bar at 298 K. This makes F4_MIL-140A(Ce) exceptionally selective for CO2 over N2: the calculated selectivity, according to the ideal adsorbed solution theory for a 0.15:0.85 mixture at 1 bar and 293 K, is higher than 1900, among the highest ever reported for metal–organic frameworks. The calculated isosteric heat of CO2 adsorption is in the range of 38–40 kJ mol–1, indicating a strong physisorptive character.
Data Access Statement:Crystallographic data presented in this paper can be obtained free of charge from the Cambridge Crystallographic Data Centre under entries CCDC-1855704 and CCDC-1855705 via www.ccdc.cam.ac.uk/data_request/cif.
Carbon dioxide capture; Gas separations; Green synthesis; Metal−organic frameworks; Porous materials
Faculty of Science and Engineering